Abstract
During weathering and pedogenesis of carbonate rock with poor-uranium (U) and thorium (Th), U and Th present the characteristics of strong leaching (especially U) and significant residual enrichment, the cause of which is still unclear. In this paper, a weathering profile developed by dolomite in karst area of Guizhou province in southwest China was selected, which showed zonation characteristics of bedrock (Y), powdery rock (Yf), and soil layer (T1 to T12) from the bottom to up. Through the determination of the occurrence speciation of U and Th in Y and weathering profile, combined with mineralogical, geochemical characteristics, and element mass balance calculation, the constraints of U and Th speciation on the geochemical behavior of U and Th during the weathering of carbonate rock were revealed. The results proved that U and Th in Y preferentially existed in acid insoluble phase, for example, the contents of U and Th in Y were 0.90 mg·kg−1 and 0.28 mg·kg−1, respectively, while those in acid insoluble matter were 2.34 mg·kg−1 and 2.57 mg·kg−1, respectively, but because the mass percentage of acid insoluble matter was extremely low (0.95%), the mass percentages of U and Th in the acid soluble phase in the whole rock were absolutely superior (96% of U and 86% Th). The U and Th in the acid soluble phase of Y were mainly adsorbed on the crystal surface of carbonate minerals or existed in the cement, and the U and Th in the carbonate lattice only accounted for a small proportion. From Y to Yf with the initial dissolution, U and Th released from the surface of carbonate minerals and cements were in carbonate-rich alkaline environment, and these portions of U and Th were leached out, resulting in strong loss of U and Th in the Yf (the loss rates are 83% of U and 65% of Th, respectively). From the Yf to the overlying soil layer T1, the carbonate components were completely dissolved, and the U and Th released from the carbonate lattice showed different behaviors, where U was completely leached and Th tended to stay in the weathered residue. Thus, in the soil layer T1 formed by Y or Yf , the residual U was the inheritance of the U in the acid insoluble phase of Y; For Th, it not only inherited the Th of acid insoluble phase of Y, but also superimposed the Th from carbonate lattice in Y. On the other hand, during the evolution process from Y to Yf and to soil layer T1, with the dissolution of carbonate, the acid insoluble phase also showed a significant tendency of chemical weathering. However, the U and Th in the Y acid insoluble phase were not leached with the decomposition of the acid insoluble phase but were redistributed among the residual phases. For the geochemical behaviors of U and Th in the evolution of soil profile (T1~T12), they were subjected to the occurrence speciation of U and Th in T1 and the change of U and Th occurrence speciation with the upward direction of soil profile. The U and Th released from the carrier minerals were mainly redistributed among the residual solid phases, which weakened the intensity of their further loss. This study deepens the understanding of the geochemical behavior of radionuclides in karst environment and provides reference for the treatment of radioactive pollution in karst areas.
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This study was supported by the National Natural Science Foundation of China (grant no. 41373115).
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All authors contributed to the study conception and design. Qiang Ma: data curation, formal analysis, writing—original draft. Bing-jie Zhou: methodology, data curation, formal analysis. Zhi-gang Feng: conceptualization, methodology, funding acquisition, writing—review and editing. Xiao-long Wang: formal analysis, visualization. Rong Chen: investigation, methodology. Pei-shan Li: investigation, data curation. Chong Huang: investigation, data curation.
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Highlights
1. During weathering and pedogenesis of carbonate rock, U and Th presented the characteristics of low content of background values, strong leaching (especially U), and high enrichment.
2. U and Th in bedrock preferentially occured in acid insoluble phase, but their mass percentages in acid soluble phase are absolutely dominant. They in acid soluble phase were mainly adsorbed on the surface of carbonate minerals or occur in cements.
3. By preliminary dissolution from bedrock to powdery rock layer, U and Th released from the carbonate mineral surface or cements were fully leached under alkaline conditions rich in carbonate.
4. During the rock-soil interface reaction, with full dissolution of carbonate components, U hosted in carbonate lattice was also leached, while Th was mainly absorbed in the residues.
5. The evolution of the residues rich in U and Th, formed by the rock-soil interface reaction, led to their enrichment in soil layer.
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Ma, Q., Zhou, Bj., Feng, Zg. et al. Geochemical behaviors of uranium and thorium during weathering and pedogenesis of carbonate rock: constraint from their speciation. Environ Sci Pollut Res 30, 95348–95366 (2023). https://doi.org/10.1007/s11356-023-29007-5
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DOI: https://doi.org/10.1007/s11356-023-29007-5